No abstract

Solution processing of semiconductors is highly promising for the high-throughput production of cost-effective electronics and optoelectronics. Although hybrid perovskites have potential in various device applications, challenges remain in the development of high-quality materials with simultaneously improved processing reproducibility and scalability. Here, we report a liquid medium annealing (LMA) technology that creates a robust chemical environment and constant heating field to modulate crystal growth over the entire film. Our method produces films with high crystallinity, fewer defects, desired stoichiometry, and overall film homogeneity. The resulting perovskite solar cells (PSCs) yield a stabilized power output of 24.04% (certified 23.7%, 0.08 cm2) and maintain 95% of their initial power conversion efficiency (PCE) after 2000 hours of operation. In addition, the 1-cm2 PSCs exhibit a stabilized power output of 23.15% (certified PCE 22.3%) and keep 90% of their initial PCE after 1120 hours of operation, which illustrates their feasibility for scalable fabrication. LMA is less climate dependent and produces devices in-house with negligible performance variance year round. This method thus opens a new and effective avenue to improving the quality of perovskite films and photovoltaic devices in a scalable and reproducible manner.

Organic spacer cations in layered 2D (A1)2(A2)n−1BnX3n+1 (where A1 is an organic cation acting as a spacer between the perovskite layers, A2 is a monovalent cation, e.g., Cs+,CH3NH3+, CH(NH2)2+) perovskite materials improve the long‐term stability of the resulting solar cells, but hamper their power conversion efficiency due to poor carrier generation/transportation. Rational guidelines are thus required to enable the design of organic spacer cations. Herein, mixed A1 cations are employed in layered 2D perovskites to investigate the interplay between alkylamine cations and unsaturated alkylamine cations. It is revealed that alkylamine spacer cations are able to facilitate precursor assembly, which results in the orientated growth of perovskite crystals. Unsaturated alkylamine cations further lead to reduced exciton binding energy, which improves carrier pathway in the 2D perovskites. By mixing both cations, substantially improved open circuit voltage is observed in the resultant photovoltaic cells with the efficiency of 15.46%, one of the highest one based on (A1)2(A2)3Pb4I13 layered 2D perovskites. The generality of the design principle is further extended to other cation combinations.

Developing a single-phase self-rectifying memristor with the continuously tunable feature is structurally desirable and functionally adaptive to dynamic environmental stimuli variations, which is the pursuit of further smart memristors and neuromorphic computing. Herein, we report a van der Waals ferroelectric CuInP2S6 as a single memristor with superior continuous modulation of current and self-rectifying to different bias stimuli (sweeping speed, direction, amplitude, etc.) and external mechanical load. The synergetic contribution of controllable Cu+ ions migration and interfacial Schottky barrier is proposed to dynamically control the current flow and device performance. These outstanding sensitive features make this material possible for being superior candidate for future smart memristors with bidirectional operation mode and strong recognition to input faults and variations.

Van der Waals (vdW) layered materials have rather weaker interlayer bonding than the intralayer bonding, therefore the exfoliation along the stacking direction enables the achievement of monolayer or few layers vdW materials with emerging novel physical properties and functionalities. The ferroelectricity in vdW materials recently attracts renewed interest for the potential use in high-density storage devices. As the thickness going thinner, the competition between the surface energy, depolarization field and interfacial chemical bonds may give rise to the modification of ferroelectricity and crystalline structure, which has limited investigations.In this work, combining the piezoresponse force microscope scanning, contact resonance imaging, we report the existence of the intrinsic in-plane polarization in vdW ferroelectrics CuInP 2 S 6 (CIPS) single crystals, whereas below a critical thickness between 90-100 nm, the inplane polarization disappears. The Young's modulus also shows an abrupt stiffness at the critical thickness. Based on the density functional theory calculations, we ascribe these behaviors to a structural phase transition from monoclinic to trigonal structure, which is further

Recent realizations of ultrathin freestanding perovskite oxides offer a unique platform to probe novel properties in two-dimensional oxides. Here, we observe a giant flexoelectric response in freestanding BiFeO3 and SrTiO3 in their bent state arising from strain gradients up to 3.5 × 107 m−1, suggesting a promising approach for realizing ultra-large polarizations. Additionally, a substantial change in membrane thickness is discovered in bent freestanding BiFeO3, which implies an unusual bending-expansion/shrinkage effect in the ferroelectric membrane that has never been seen before in crystalline materials. Our theoretical model reveals that this unprecedented flexural deformation within the membrane is attributable to a flexoelectricity–piezoelectricity interplay. The finding unveils intriguing nanoscale electromechanical properties and provides guidance for their practical applications in flexible nanoelectromechanical systems.

Symmetry is highly relevant with various quantities and phenomena in physics. While the translational symmetry breaks at the edges of two-dimensional hexagonal crystalline flakes, it is usually associated with the breaking of central inversion symmetry that is yet to be observed in terms of physical properties. Here, we report an experiment–theory joint study on in-plane compressed single-crystal monolayer WS2 flakes. Although the flakes show a hexagonal appearance with a C6 symmetry, our density functional theory calculations predict that their in-plane strain, geometric structure, work-function, energy bandgap, and mechanical modulus are nonequivalent among the triangular regions with different edge terminations at the atomic scale, and the flakes exhibit self-patterns with a C3 symmetry. Such nonequivalence of physical properties and concomitant self-patterns persist even in a 50 μm-sized monolayer WS2, observed using atomic force microscopy. This indicates that the symmetry arising from the atomic geometry could preserve up to tens of microns for both geometric and properties of the flake, regardless of its mesoscopic geometry, i.e., C6 here. Such a detectable mesoscopic scale and symmetric nano- to mesoscale patterns provide promising building blocks for 2D materials and devices and also allow edge terminations of 2D flakes to be directly distinguished.

The strain has been employed for controlled modification of electronical and mechanical properties of two-dimensional (2D) materials. However, the thermal strain-engineered behaviors of the CVD-grown MoS 2 have not been systematically explored. Here, we investigated the strain-induced structure and properties of CVD-grown triangular MoS 2 flakes by several advanced atomic force microscopy. Two different kinds of flakes with sharp-corner or vein-like nanostructures are experimentally discovered due to the size-dependent strain behaviors. The critical size of these two kinds of flakes can be roughly estimated at∼17 μm. Within the small flakes, the sharp-corner regions show specific strain-modified properties due to the suffering of large tensile strain. While in the large MoS 2 flakes, the complicated vein-like nanoripple structures were formed due to the interface slipping process under the larger tensile strain. Our work not only demonstrates the size-specific strain behaviors of MoS 2 flakes but also sheds light on the artificial design and preparation of strain-engineered nanostructures for the devices based on the 2D materials.